Imaging nanoscale molecular binding in functionalized graphene via tip-enhanced Raman spectroscopy

Author:

You Xiao12ORCID,Huang Chiung-Wei3ORCID,Vinodgopal Kizhanipuram4,Atkin Joanna M.3ORCID

Affiliation:

1. Department of Applied Physical Science, University of North Carolina at Chapel Hill 1 , Chapel Hill, North Carolina 27599, USA

2. Department of Engineering, Westlake University 2 , Hangzhou, China

3. Department of Chemistry, University of North Carolina at Chapel Hill 3 , Chapel Hill, North Carolina 27599, USA

4. Department of Chemistry, North Carolina Central University 4 , Durham, North Carolina 27707, USA

Abstract

Surface functionalization of low-dimensional nanomaterials offers a means to tailor their optoelectronic and chemical characteristics. However, functionalization reactions are sensitive to the inherent surface features of nanomaterials, such as defects, grain boundaries, and edges. Conventional optical characterization methods, such as Raman spectroscopy, have limited sensitivity and spatial resolution and, therefore, struggle to visualize reaction sites and chemical species. Here, we demonstrate the capability of spatially and chemically sensitive tip-enhanced Raman spectroscopy imaging to map the distribution of molecules in covalently functionalized graphene. Hyperspectral vertex component analysis and density functional theory are necessary to interpret the nature of binding sites and extract information from the spatially and spectrally heterogeneous datasets. Our results clarify the origin of heterogeneous surface functionalization, resolving preferential binding at edges and defects. This work demonstrates the potential of nanospectroscopic tools combined with unsupervised learning to characterize complex, partially ordered optoelectronic nanomaterials.

Funder

National Science Foundation

Publisher

AIP Publishing

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